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Spectral phase optimization of femtosecond laser pulses for narrow-band, low-background nonlinear spectroscopy

Vadim V. Lozovoy, Janelle C. Shane, Bingwei Xu, and Marcos Dantus

Open Access Open Access

Abstract

We use experimental search space mapping to examine the problem of selective nonlinear excitation with binary phase shaped femtosecond laser pulses. The search space maps represent a graphical view of all the possible solutions to the selective nonlinear excitation problem along with their experimental degrees of success. Using the information learned from these maps, we generate narrow lines with low background in second harmonic generation and stimulated Raman scattering spectra.

©2005 Optical Society of America

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Supplementary Material (4)

Media 1: GIF (896 KB)     
Media 2: GIF (714 KB)     
Media 3: AVI (809 KB)     
Media 4: AVI (446 KB)     

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Figures (3)
Fig. 1.
Fig. 1. Nonlinear spectra of phase modulated pulses. The dashed line is the spectrum of a Gaussian transform-limited (flat spectral phase) pulse. (a) Maximization or minimization of nonlinear spectra at a selected frequency. (b) Generation of a narrow peak at a selected frequency with low background (the goal of this project).

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Fig. 2.
Fig. 2. Experimental mapping of selective SHG (left) and SRS (right) at the center of the spectrum (see Fig. 1(b). X and y coordinates are the decimal representations of the left and right halves of the binary phase sequences, respectively, and color as z coordinate is the experimentally measured signal to background ratio of nonlinear excitation. Here, phase sequences with high S/B ratios are shown in red, while sequences with low S/B ratios are shown in black. Arrows point to the locations of the global maxima. [Media 1] [Media 2]

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Fig. 3.
Fig. 3. Experimental generation (dots) and simulation (red) of narrow-band and low-background nonlinear fields using optimized binary phase functions. (a) and (b) Phase (black) and amplitude (red) modulation was imprinted with the SLM on a broad fundamental pulse. (c) SHG spectrum measured with a nonlinear crystal. (d) SRS spectrum recorded as the Fourier transform of the autocorrelation trace using a collinear Michelson interferometer. [Media 3] [Media 4]

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